Comparative Study of CH Stretch and Bend Vibrations in Methane Activation on Ni(100) and Ni(111)

L. B. F. Juurlink, R. R. Smith, D. R. Killelea, and A. L. Utz
Phys. Rev. Lett. 94, 208303 – Published 25 May 2005

Abstract

State-resolved measurements on clean Ni(100) and Ni(111) surfaces quantify the reactivity of CH4 excited to v=3 of the ν4 bend vibration. A comparison with prior data reveals that 3ν4 is significantly less effective than the ν3 CH stretch at promoting dissociative chemisorption, even though 3ν4 contains 30% more energy. These results contradict statistical theories of gas-surface reactivity, provide clear evidence for vibrational mode specificity in a gas-surface reaction, and point to a central role for CH stretching motion along the reaction path to dissociative chemisorption.

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  • Received 2 December 2004

DOI:https://doi.org/10.1103/PhysRevLett.94.208303

©2005 American Physical Society

Authors & Affiliations

L. B. F. Juurlink

  • Leiden Institute of Chemistry, Gorlaeus Laboratories, Leiden University, 2300 RA Leiden, The Netherlands

R. R. Smith, D. R. Killelea, and A. L. Utz

  • Department of Chemistry and W. M. Keck Foundation Laboratory, Tufts University, Medford, Massachusetts 02155, USA

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Vol. 94, Iss. 20 — 27 May 2005

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